Strain enhances the activity of molecular electrocatalysts via carbon nanotube supports

Jianjun Su, Charles B. Musgrave, Yun Song, Libei Huang, Yong Liu, Geng Li, Yinger Xin, Pei Xiong, Meng-jung Li, Haoran Wu, Minghui Zhu, Hao Ming Chen, Jianyu Zhang, Hanchen Shen, Ben Zhong Tang, Marc Robert, William A. Goddard, Ruquan Ye

Research output: Journal article publicationJournal articleAcademic researchpeer-review

74 Citations (Scopus)

Abstract

Support-induced strain engineering is useful for modulating the properties of two-dimensional materials. However, controlling strain of planar molecules is technically challenging due to their sub-2 nm lateral size. Additionally, the effect of strain on molecular properties remains poorly understood. Here we show that carbon nanotubes (CNTs) are ideal substrates for inducing optimum properties through molecular curvature. In a tandem-flow electrolyser with monodispersed cobalt phthalocyanine (CoPc) on single-walled CNTs (CoPc/SWCNTs) for CO2 reduction, we achieve a methanol partial current density of >90 mA cm−2 with >60% selectivity, surpassing wide multiwalled CNTs at 16.6%. We report vibronic and X-ray spectroscopies to unravel the distinct local geometries and electronic structures induced by the strong molecule–support interactions. Grand canonical density functional theory confirms that curved CoPc/SWCNTs improve *CO binding to enable subsequent reduction, whereas wide multiwalled CNTs favour CO desorption. Our results show the important role of SWCNTs beyond catalyst dispersion and electron conduction. [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)818-828
Number of pages11
JournalNature Catalysis
Volume6
Issue number9
DOIs
Publication statusPublished - Aug 2023

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

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